| 1. |
- Goudsmit-Harzevoort, Barbara, et al.
(författare)
-
The Relationship Between the Global Mean Deep-Sea and Surface Temperature During the Early Eocene
- 2023
-
Ingår i: Paleoceanography and Paleoclimatology. - 2572-4517 .- 2572-4525. ; 38:3
-
Tidskriftsartikel (refereegranskat)abstract
- Estimates of global mean near-surface air temperature (global SAT) for the Cenozoic era rely largely on paleo-proxy data of deep-sea temperature (DST), with the assumption that changes in global SAT covary with changes in the global mean deep-sea temperature (global DST) and global mean sea-surface temperature (global SST). We tested the validity of this assumption by analyzing the relationship between global SST, SAT, and DST using 25 different model simulations from the Deep-Time Model Intercomparison Project simulating the early Eocene Climatic Optimum (EECO) with varying CO2 levels. Similar to the modern situation, we find limited spatial variability in DST, indicating that local DST estimates can be regarded as a first order representative of global DST. In line with previously assumed relationships, linear regression analysis indicates that both global DST and SAT respond stronger to changes in atmospheric CO2 than global SST by a similar factor. Consequently, this model-based analysis validates the assumption that changes in global DST can be used to estimate changes in global SAT during the early Cenozoic. Paleo-proxy estimates of global DST, SST, and SAT during EECO show the best fit with model simulations with a 1,680 ppm atmospheric CO2 level. This matches paleo-proxies of EECO atmospheric CO2, indicating a good fit between models and proxy-data.
|
|
| 2. |
- Wang, Xi, et al.
(författare)
-
Self-Constructed Multiple Plasmonic Hotspots on an Individual Fractal to Amplify Broadband Hot Electron Generation
- 2021
-
Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 15:6, s. 10553-10564
-
Tidskriftsartikel (refereegranskat)abstract
- Plasmonic nanoparticles are ideal candidates for hot-electron-assisted applications, but their narrow resonance region and limited hotspot number hindered the energy utilization of broadband solar energy. Inspired by tree branches, we designed and chemically synthesized silver fractals, which enable self-constructed hotspots and multiple plasmonic resonances, extending the broadband generation of hot electrons for better matching with the solar radiation spectrum. We directly revealed the plasmonic origin, the spatial distribution, and the decay dynamics of hot electrons on the single-particle level by using ab initio simulation, dark-field spectroscopy, pump–probe measurements, and electron energy loss spectroscopy. Our results show that fractals with acute tips and narrow gaps can support broadband resonances (400–1100 nm) and a large number of randomly distributed hotspots, which can provide unpolarized enhanced near field and promote hot electron generation. As a proof-of-concept, hot-electron-triggered dimerization of p-nitropthiophenol and hydrogen production are investigated under various irradiations, and the promoted hot electron generation on fractals was confirmed with significantly improved efficiency.
|
|
| 3. |
- Zhang, X., et al.
(författare)
-
Plasmon-driven sequential chemical reactions in an aqueous environment
- 2014
-
Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322 .- 2045-2322. ; 4
-
Tidskriftsartikel (refereegranskat)abstract
- Plasmon-driven sequential chemical reactions were successfully realized in an aqueous environment. In an electrochemical environment, sequential chemical reactions were driven by an applied potential and laser irradiation. Furthermore, the rate of the chemical reaction was controlled via pH, which provides indirect evidence that the hot electrons generated from plasmon decay play an important role in plasmon-driven chemical reactions. In acidic conditions, the hot electrons were captured by the abundant H+ in the aqueous environment, which prevented the chemical reaction. The developed plasmon-driven chemical reactions in an aqueous environment will significantly expand the applications of plasmon chemistry and may provide a promising avenue for green chemistry using plasmon catalysis in aqueous environments under irradiation by sunlight.
|
|
| 4. |
- Zhang, Yurui, et al.
(författare)
-
Early Eocene Ocean Meridional Overturning Circulation : The Roles of Atmospheric Forcing and Strait Geometry
- 2022
-
Ingår i: Paleoceanography and Paleoclimatology. - 2572-4517 .- 2572-4525. ; 37:3
-
Tidskriftsartikel (refereegranskat)abstract
- Here, we compare the ocean overturning circulation of the early Eocene (47–56 Ma) in eight coupled climate model simulations from the Deep-Time Model Intercomparison Project (DeepMIP) and investigate the causes of the observed inter-model spread. The most common global meridional overturning circulation (MOC) feature of these simulations is the anticlockwise bottom cell, fed by sinking in the Southern Ocean. In the North Pacific, one model (GFDL) displays strong deepwater formation and one model (CESM) shows weak deepwater formation, while in the Atlantic two models show signs of weak intermediate water formation (MIROC and NorESM). The location of the Southern Ocean deepwater formation sites varies among models and relates to small differences in model geometry of the Southern Ocean gateways. Globally, convection occurs in the basins with smallest local freshwater gain from the atmosphere. The global MOC is insensitive to atmospheric CO2 concentrations from 1× (i.e., 280 ppm) to 3× (840 ppm) pre-industrial levels. Only two models have simulations with higher CO2 (i.e., CESM and GFDL) and these show divergent responses, with a collapsed and active MOC, respectively, possibly due to differences in spin-up conditions. Combining the multiple model results with available proxy data on abyssal ocean circulation highlights that strong Southern Hemisphere-driven overturning is the most likely feature of the early Eocene. In the North Atlantic, unlike the present day, neither model results nor proxy data suggest deepwater formation in the open ocean during the early Eocene, while the evidence for deepwater formation in the North Pacific remains inconclusive.
|
|
| 5. |
- Cui, L., et al.
(författare)
-
Plasmon-driven dimerization via S-S chemical bond in an aqueous environment
- 2014
-
Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322 .- 2045-2322. ; 4
-
Tidskriftsartikel (refereegranskat)abstract
- The surface-enhanced Raman scattering (SERS) spectra of thioanisole are experimentally investigated in an electrochemical environment in this study. Two Raman peaks, which depend strongly not only on electric potential but also on the local surface plasmon resonances (LSPR), have been observed. Theoretical calculations reveal that thioanisole is first dissociated from thiophenol via the S-CH3 bond; plasmons then drive the dimerisation of thiophenol via the S-S bond, which is strongly potential dependent. One Raman peak corresponds to the S-S vibrational mode of the thiophenol dimer, and the other corresponds to the asymmetric C-C stretching modes of the benzenyl of the thiophenol dimer. The potential-dependent two Raman modes is the potential-dependent dimerisation dynamics of thiophenol via the S-S bond. Our experimental findings provide insight into the structural elucidation of adsorbed molecules and molecular surface reaction dynamics.
|
|
| 6. |
- Fang, Yurui, et al.
(författare)
-
Branched Silver Nanowires as Controllable Plasmon Routers
- 2010
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6992 .- 1530-6984. ; 10:5, s. 1950-1954
-
Tidskriftsartikel (refereegranskat)abstract
- Using polarization dependent scattering spectroscopy, we investigate plasmon propagation on branched silver nanowires. By controlling the polarization of the incident laser light, the wire plasmons can be routed into different wire branches and result in light emission from the corresponding wire ends. This routing behavior is found to be strongly dependent on the wavelength of light. Thus for certain incident polarizations, light of different wavelength will be routed into different branches. The branched nanowire can thus serve as a controllable router and multiplexer in integrated plasmonic circuits.
|
|
| 7. |
- Fang, Yurui, 1983, et al.
(författare)
-
High vacuum tip-enhanced Raman spectroscope based on a scanning tunneling microscope
- 2016
-
Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 1089-7623 .- 0034-6748. ; 87:3, s. 033104-
-
Tidskriftsartikel (refereegranskat)abstract
- In this paper, we present the construction of a high-vacuum tip-enhanced Raman spectroscopy (HV-TERS) system that allows in situ sample preparation and measurement. A detailed description of the prototype instrument is presented with experimental validation of its use and novel ex situ experimental results using the HV-TERS system. The HV-TERS system includes three chambers held under a 10(-7) Pa vacuum. The three chambers are an analysis chamber, a sample preparation chamber, and a fast loading chamber. The analysis chamber is the core chamber and contains a scanning tunneling microscope (STM) and a Raman detector coupled with a 50 x 0.5 numerical aperture objective. The sample preparation chamber is used to produce single-crystalline metal and sub-monolayer molecular films by molecular beam epitaxy. The fast loading chamber allows ex situ preparation of samples for HV-TERS analysis. Atomic resolution can be achieved by the STM on highly ordered pyrolytic graphite. We demonstrate the measurement of localized temperature using the Stokes and anti-Stokes TERS signals from a monolayer of 1,2-benzenedithiol on a gold film using a gold tip. Additionally, plasmonic catalysis can be monitored label-free at the nanoscale using our device. Moreover, the HV-TERS experiments show simultaneously activated infrared and Raman vibrational modes, Fermi resonance, and some other non-linear effects that are not observed in atmospheric TERS experiments. The high spatial and spectral resolution and pure environment of high vacuum are beneficial for basic surface studies.
|
|
| 8. |
- Fang, Yurui, 1983, et al.
(författare)
-
Near field plasmonic gradient effects on high vacuum tip-enhanced Raman spectroscopy
- 2015
-
Ingår i: Physical Chemistry Chemical Physics. - : Royal Society of Chemistry (RSC). - 1463-9084 .- 1463-9076. ; 17:2, s. 783-794
-
Tidskriftsartikel (refereegranskat)abstract
- Near field gradient effects in high vacuum tip-enhanced Raman spectroscopy (HV-TERS) are a recent developing ultra-sensitive optical and spectral analysis technology on the nanoscale, based on the plasmons and plasmonic gradient enhancement in the near field and under high vacuum. HV-TERS can not only be used to detect ultra-sensitive Raman spectra enhanced by surface plasmon, but also to detect clear molecular IR-active modes enhanced by strongly plasmonic gradient. Furthermore, the molecular overtone modes and combinational modes can also be experimentally measured, where the Fermi resonance and Darling-Dennison resonance were successfully observed in HV-TERS. Theoretical calculations using electromagnetic field theory firmly supported experimental observation. The intensity ratio of the plasmon gradient term over the linear plasmon term can reach values greater than 1. Theoretical calculations also revealed that with the increase in gap distance between tip and substrate, the decrease in the plasmon gradient was more significant than the decrease in plasmon intensity, which is the reason that the gradient Raman can be only observed in the near field. Recent experimental results of near field gradient effects on HV-TERS were summarized, following the section of the theoretical analysis.
|
|
| 9. |
- Gao, Yongzhi, et al.
(författare)
-
Potent Inhibition of Nicotinamide N-Methyltransferase by Alkene-Linked Bisubstrate Mimics Bearing Electron Deficient Aromatics
- 2021
-
Ingår i: Journal of Medicinal Chemistry. - : American Chemical Society (ACS). - 0022-2623 .- 1520-4804. ; 64:17, s. 12938-12963
-
Tidskriftsartikel (refereegranskat)abstract
- Nicotinamide N-methyltransferase (NNMT) methylates nicotinamide (vitamin B3) to generate 1-methylnicotinamide (MNA). NNMT overexpression has been linked to a variety of diseases, most prominently human cancers, indicating its potential as a therapeutic target. The development of small-molecule NNMT inhibitors has gained interest in recent years, with the most potent inhibitors sharing structural features based on elements of the nicotinamide substrate and the S-adenosyl-L-methionine (SAM) cofactor. We here report the development of new bisubstrate inhibitors that include electron-deficient aromatic groups to mimic the nicotinamide moiety. In addition, a trans-alkene linker was found to be optimal for connecting the substrate and cofactor mimics in these inhibitors. The most potent NNMT inhibitor identified exhibits an IC50 value of 3.7 nM, placing it among the most active NNMT inhibitors reported to date. Complementary analytical techniques, modeling studies, and cell-based assays provide insights into the binding mode, affinity, and selectivity of these inhibitors.
|
|
| 10. |
- Huang, Y. Z., et al.
(författare)
-
Nanowire-supported plasmonic waveguide for remote excitation of surface-enhanced Raman scattering
- 2014
-
Ingår i: Light: Science and Applications. - : Springer Science and Business Media LLC. - 2047-7538 .- 2095-5545. ; 3, s. Art. no. e199-
-
Forskningsöversikt (refereegranskat)abstract
- Due to its amazing ability to manipulate light at the nanoscale, plasmonics has become one of the most interesting topics in the field of light-matter interaction. As a promising application of plasmonics, surface-enhanced Raman scattering (SERS) has been widely used in scientific investigations and material analysis. The large enhanced Raman signals are mainly caused by the extremely enhanced electromagnetic field that results from localized surface plasmon polaritons. Recently, a novel SERS technology called remote SERS has been reported, combining both localized surface plasmon polaritons and propagating surface plasmon polaritons (PSPPs, or called plasmonic waveguide), which may be found in prominent applications in special circumstances compared to traditional local SERS. In this article, we review the mechanism of remote SERS and its development since it was first reported in 2009. Various remote metal systems based on plasmonic waveguides, such as nanoparticle-nanowire systems, single nanowire systems, crossed nanowire systems and nanowire dimer systems, are introduced, and recent novel applications, such as sensors, plasmon-driven surface-catalyzed reactions and Raman optical activity, are also presented. Furthermore, studies of remote SERS in dielectric and organic systems based on dielectric waveguides remind us that this useful technology has additional, tremendous application prospects that have not been realized in metal systems.
|
|
